Abstract
Macro-porous alumina was used as a support for a pellet-type Cu-based desulfurization sorbent in the gas purification process for producing blue hydrogen by the gasification of petroleum coke. The effects of the macro-porous alumina on the pellet-type sorbents in reducing the gas diffusion resistance into the pores were investigated. The results showed that the macro-porous alumina enhances the diffusion resistance, resulting in an improved sulfur capacity of CuO absorbents. Such effects were more significant on the pellet type CuO absorbents than the powder type. In addition, CO production was observed experimentally during the desulfurization reaction of carbonyl sulfide (COS) at low temperatures (~473 K). Density functional theory calculations were also performed to understand the kinetics of desulfurization and CO production. The simulation results predicted that the kinetics of desulfurization is strongly affected by the local surface environment. The CO generated from C–O bond breaking from COS had a lower adsorption energy than the CO2 formation. These results suggest that the Cu-based desulfurization sorbent has potential catalytic activity for producing CO from COS dissociation.
Highlights
Global warming is putting a brake on the continuous use of fossil fuels used in industry
The XRD peak intensity of CuO supported on the γ-alumina surface was stronger than that on the macro-porous alumina surface
This study focused on other surface environments, including a defect surface and a sulfurized surface potentially generated during the desulfurization reactions to resolve the inconsistency
Summary
Global warming is putting a brake on the continuous use of fossil fuels used in industry. Macro-porous materials were synthesized using polymer beads as templates for catalyst materials, such as silica, titania, and alumina [22,23,24,25] With these γ-alumina and macro-porous alumina supports, pellet and powder types of Cu-based absorbents were prepared. The experimental results showed that macro-porous alumina-based CuO absorbents provide better sulfur capacity than the γ alumina-based CuO absorbents (~1.3 times higher sulfur capacity) This suggests that the enhancement of gas diffusion resistance by structural modification improves the sulfur capacity. The stability of CO generated from the C–O bond cleavage of COS was lower than the CO2 formation energy This suggests that CO prefers to desorb from the surface rather than form CO2. 2.3Fi.gPurreep2a.rPaFrtigoioucneredou2f.rCePrufooOcre/tdhAuelruepmrfoeirpntahareaAtpiobresnpooarrfbametnioatncbrooyfpmIomraocpurrosepgaolnruoamutisionanaluMbmyientteahmbodypltaetme pmlaettehmodet.hod. 2.3.CPureOpawraatisondeopf 2Co.3su.iOtPe/rdAeploaurnmattiinhonaeAomfbCasuocrOrbo/eA-npltuobmryoinIumasAparblesugonmrbaeitnniotanbayMnImdetphcrooedgmnamtieonrcMiaelthaoldumina powder bssapobpuupriyoeppbssaobngpplpwuupryieolidangppermpplpwdnleiodtaoopepmr-ripendxetorrCtoco.-ryiittrrpexrtrcumie.AbepyrttrnitdeOgmiiboeApfeatngndtginoeotngfaedfawneattoonrtdfabheelttaeonarybherirseγkltmsrnrysoieγfkmn-n6oCgdoraf-nC6e0gorbaperluca0bep0urulpebssapobpecmuoa0deuuepmnpriymoeolo°pdnnpmgllipplpw◦tosrCpelnlidrtiiaopeppCieermilnwtneptgdn.elwnoCtdtsceooecd.g-sareipex,auTrarrtiuduc.,aTbirrynittraasnbrhOmieaArsanbeyhpnontgsnnsgdynegnpioipfeeoangoni,wdtd,tndadtrotrrareadrhfaraheatdete,aoan,rmdabnhmeahnleatpepsardtyaitrsedγkpdapedmeaneaaaaodiCfn-tip6tCCpgnrcrocmranae-uau-e0euberprtrrrltgupuppgca0susrodroooaedOemoodieipeOp-mnpc,xl-xwnnw,°spplaai/prrrtoarCieiina/ggipoottmoteomaAaAloswtngeee.sdsxce-rtxtaardaddps,aluToraeleaiisboi2nhm2aatsrourrrmhhtonOOryCue,goseConn,responoiaol,listodwat3d3uiayurtttywararahttutadeeaa-aa,mhlr-nnewae5bplurwsdtlnbb5bayeypdlaeuyaaaimyiassawatpCnnamvcriswm5a-ouosslnevrtre5sgiuuatpresrrFonaodwtsdaibcieOpbmF%dwcsi-nxwhna,cua%gpetrrehiiaa/agautoiomgatnwuuAoan%esoanbp-txuwu%rtabrdmotpepflasaasoiee2mwrrsmohtofsoOrewmaudeC-,aeooo3forredsmvalsa-3nioburt.fyawec3vbtestaaaavbdu-eatsec.evbyarwrlnbb5hpaelnslauytipyacypcsaeynrhraaltiwmaooipsonceidvr5sluntylaeewrmceirputoaibmFduwldnsne(awpcmear%ca5ehmilatmuagxtearal(ns,oaaesiueu5twu%tlrbeno1tprixsolrpde,msll.rsru0faewuatioreciuod1opcr,Tdsbmll.-assir0fauaiol3aeauhieynvbcvTbsct,.evbonsslaealdeeaeyathweyahinpvdanrhstlornpaeccieerleityhaawean1mueomiozdasruldnsawse5pmmrecitaamezmoaam1eada(atwaestsm5telitu5rrdnxsholnee,osediutaanttedrwonid1atapirurlln%.drthn0uioedtetiucpnctTbmod,nooodssaii),alya%ahotne.ivfrtedttaoaenlgoaemweAeoodChw,nn)nadssarfir.faefdldiuataenagaatAuzmam1anCnneeasOsietas5mnafecrrfetotdduaianttwtanurindeahOineinaentcrdtnoaai%tntedtpomood,)or.faaegawACnnasffd (a)
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